We retrospectively evaluated the altered biomechanics of the talus in 15 adult patients (7 males, 8 females) with chronic lateral ankle instability when the ankle joint moved actively from full dorsiflexion to full plantarflexion under a non-weight bearing condition. CT images were taken for the unstable ankle and the contralateral normal (control) ankle. Three-dimensional surface models of both ankle joints were reconstructed from the CT data, and we used a computer simulation program to compare both ankle motions of inversion/eversion in the coronal plane, plantarflexion/dorsiflexion in the sagittal plane, and internal rotation/external rotation in the axial plane. This evaluation method provides in vivo, dynamic, and 3D results of ankle motion. In the ankles with chronic lateral instability and the controls, the average talar rotational movement of inversion (+)/eversion (−) was 19.0° and 15.5° and the internal rotation (+)/external rotation (−) was 30.4° and 20.7°, respectively. Paired t-tests revealed significant differences in the amount of inversion (+)/eversion (−) (p=0.012) and internal rotation (+)/external rotation (−) (p<0.001) between unstable and normal ankle joints. The difference of mean rotational movement in internal rotation (9.7°) was greater than that of inversion (3.5°). Rotational instability should be considered when evaluating chronic lateral ankle instability.